Article
Chemistry, Physical
Antonis Vamvakeros, Dorota Matras, Thomas E. Ashton, Alan A. Coelho, Hongyang Dong, Dustin Bauer, Yaroslav Odarchenko, Stephen W. T. Price, Keith T. Butler, Olof Gutowski, Ann-Christin Dippel, Martin von Zimmerman, Jawwad A. Darr, Simon D. M. Jacques, Andrew M. Beale
Summary: Synchrotron high-energy X-ray diffraction computed tomography has been employed to investigate the cycling performance of commercial cylindrical Li-ion batteries for the first time, showing its potential in detecting internal battery structure and chemical composition.
Article
Multidisciplinary Sciences
Alice J. Merryweather, Christoph Schnedermann, Quentin Jacquet, Clare P. Grey, Akshay Rao
Summary: The key to advancing lithium-ion battery technology, especially fast charging, lies in understanding dynamic processes in functioning materials under realistic conditions in real time. A laboratory-based optical interferometric scattering microscope was introduced to study nanoscopic lithium-ion dynamics in battery materials, allowing for high-throughput material screening. This methodology was applied to study various processes in battery materials, providing insights into battery degradation mechanisms.
Article
Chemistry, Physical
Yuxin Chen, Loraine Torres-Castro, Kuan-Hung Chen, Daniel Penley, Joshua Lamb, Mohan Karulkar, Neil P. Dasgupta
Summary: In this study, incremental capacity analysis was applied to investigate lithium plating during charging process. The results showed the correlation between lithium plating and specific IC peak, and demonstrated the applicability of IC analysis in studying lithium plating in novel cell architectures.
JOURNAL OF POWER SOURCES
(2022)
Article
Electrochemistry
Monty R. Cosby, Gia M. Carignan, Zhuo Li, Corey M. Efaw, Charles C. Dickerson, Liang Yin, Yang Ren, Bin Li, Eric J. Dufek, Peter G. Khalifah
Summary: This study demonstrates the use of operando synchrotron X-ray diffraction (XRD) to directly characterize Li metal in standard batteries. By designing appropriately configured experiments, the stripping and plating of Li metal can be effectively quantified during battery cycling. The findings show that local variations in the deposition and stripping of Li metal can be probed, and the rate of Li usage can be tracked with sufficient spatial and time resolution. The results challenge the conventional wisdom that the greatest challenges in Li metal batteries are associated with Li deposition.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Patric Berger, Hans Flandorfer
Summary: Lithium containing alloy systems, especially the ternary Li-Sb-Sn system, are studied as potential electrode materials for lithium ion batteries. Experimental results show that SbSn can uptake up to 15 at.% Li, forming Li3Sb and confirming the ternary phase Li8SbxSn3-x.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Anirudha Jena, Zizheng Tong, Behrouz Bazri, Kevin Iputera, Ho Chang, Shu-Fen Hu, Ru-Shi Liu
Summary: Solid Li-ion conductors have the potential to enhance the performance of batteries by widening the cell-potential window and improving safety features. However, the development of all-solid-state batteries (ASSBs) faces challenges such as ion transport, interface reactions, and increased cell resistance. Advanced in situ/operando techniques are being used to explore and address these challenges.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Robert Bradbury, Georg F. Dewald, Marvin A. Kraft, Tobias Arlt, Nikolay Kardjilov, Juergen Janek, Ingo Manke, Wolfgang G. Zeier, Saneyuki Ohno
Summary: The low rate-capability of solid-state lithium-sulfur batteries is a major obstacle to their development. Neutron imaging has revealed that sluggish ion transport within the composite cathode is the main reason for this limitation. Furthermore, concentrated lithium near the current collector, discovered through state-of-charge-dependent tomography, indicates a previously overlooked loss mechanism caused by sluggish ion transport.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yun Seok Choi, Gwi Ok Park, Kyoung Ho Kim, Yelim Kwon, Joonsuk Huh, Ji Man Kim
Summary: The movement of sulfur species in the cathode of a lithium-sulfur battery was observed directly through operando SAXS analysis. Micropores serve as the primary repository for sulfur before and after the electrochemical reaction, while mesopores act as the actual reaction site for sulfur species. By establishing the distinct properties of the pores, critical insights were gained for the design of advanced carbon cathode materials.
CHEMICAL COMMUNICATIONS
(2021)
Article
Energy & Fuels
Gowthami Chandra, Shreyas J. Kashyap, Sudhakara Sarma Sreedhara, Sarada Bulusu, Venu Vinod Ananthula, R. Vijay, Tata N. Rao, Anandan Srinivasan
Summary: The present study focuses on developing carbon-coated lithium iron phosphate (LFP/C) cathode material with good capacity, high atomic efficiency, and high tap density for lithium-ion battery (LIB) fabrication. Fe3O4-LFP/C showed higher atomic efficiency and tap density compared to Fe2O3-LFP/C and Fe-LFP/C. Electrochemical studies demonstrated that Fe3O4-LFP/C exhibited a high capacity of 137 mAh g-1 at 1C and retained 83% capacity after 600 cycles at 1C, indicating excellent cyclic stability. This work provides a pathway for affordable LFP synthesis for high-energy density batteries.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Chemistry, Multidisciplinary
Xiaojing Zhang, Xinyi Ge, Zhigang Shen, Han Ma, Jingshi Wang, Shuai Wang, Lei Liu, Beibei Liu, Lixin Liu, Yizhi Zhao
Summary: Water-based binders offer numerous advantages in LIB cathodes over environmentally harmful binders like PVDF. Electrodes with SA and CMC/PTFE showed outstanding performance, with enhanced kinetics capability in Li+ transfer. The use of water-based binders resulted in smaller charge-transfer resistance values, lower polarization, and enhanced conductive network coverage on LFP electrodes, indicating promising prospects for their use in LIB cathodes.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
David E. Brown, Eric J. McShane, Zachary M. Konz, Kristian B. Knudsen, Bryan D. McCloskey
Summary: In this study, operando electrochemical impedance spectroscopy was used to reliably detect the onset of Li plating on graphite electrodes in three-electrode LIBs. By cross-validating with a highly sensitive ex situ chemical titration, it was determined that this technique can detect very small amounts of plated Li. This technique can also be applied to standard two-electrode LIB systems, making it an important step toward safely implementing fast charging protocols for LIBs in EVs.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Vittorio Marangon, Luca Minnetti, Edoardo Barcaro, Jusef Hassoun
Summary: A solid polymer electrolyte with high ionic conductivity and compatibility with different cathode materials has been developed and used in solid-state lithium-metal batteries. The electrolyte shows excellent electrochemical stability, minimal overvoltage, and low interphase resistance. The cells demonstrate reversible operation at room temperature and high capacity for various cathodes. This electrolyte has potential for application in room-temperature solid polymer cells.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Energy & Fuels
Nitheesha Shaji, Feng Jiang, Jae Yoon Sung, Murugan Nanthagopal, Taehyung Kim, Byeong Jin Jeong, Soon Phil Jung, Chang Woo Lee
Summary: This study focuses on surface modification of LiFePO4 (LFP) cathode material for lithium-ion batteries (LIBs) using heteroatoms-doped carbon. The results demonstrate that the nitrogen and sulfur dual-doped carbon coating layer enhances the electrochemical activity, cycling stability, and rate capability of the NSC@LFP cathode.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Chemistry, Physical
Vairavel Mathayan, Kenji Morita, Bun Tsuchiya, Rongbin Ye, Mamoru Baba, Daniel Primetzhofer
Summary: The study demonstrates an ion beam-based analytical method with high depth resolution and sensitivity for depth profiling Li and O in thin-film batteries. Reversible Li transport from the anode to the cathode and O transport from the anode to the cathode were observed during charge and discharge cycles, while O transport was not observed in further charging and discharging processes.
MATERIALS TODAY ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Cheng-Hung Lin, Lei Wang, Steven T. King, Jianming Bai, Lisa M. Housel, Alison H. McCarthy, Mallory N. Vila, Hengwei Zhu, Chonghang Zhao, Lijie Zou, Sanjit Ghose, Xianghui Xiao, Wah-Keat Lee, Kenneth J. Takeuchi, Amy C. Marschilok, Esther S. Takeuchi, Mingyuan Ge, Yu-chen Karen Chen-Wiegart
Summary: This study utilized a multimodal approach to investigate chemical heterogeneity in WIS batteries with thick electrodes, highlighting the importance of understanding electrochemically coupled transport phenomena in determining the rate-limiting factor. Ionic diffusion was identified as the primary rate-limiting factor in the electrolyte of these batteries.
ACS CENTRAL SCIENCE
(2021)
Article
Chemistry, Physical
Kuan-Hung Chen, Vishwas Goel, Min Ji Namkoong, Markus Wied, Simon Muller, Vanessa Wood, Jeff Sakamoto, Katsuyo Thornton, Neil P. Dasgupta
Summary: This study demonstrates that by fabricating hybrid anodes with uniform mixtures of graphite and hard carbon, it is possible to achieve high-energy density and efficient fast charging in Li-ion batteries. The optimized hybrid anodes retain significantly higher specific energy after 500 cycles of fast charging compared to graphite anodes under the same conditions, making them a promising solution for electric vehicles.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Krystal Lee, Carrie Siu, Marc F. Hidalgo, Jatinkumar Rana, Mateusz Zuba, Youngmin Chung, Fredrick Omenya, Louis F. J. Piper, Hao Liu, Natasha A. Chernova, M. Stanley Whittingham
Summary: Lithium vanadyl phosphate has a theoretical capacity of 305 mA h g(-1) but faces challenges in capacity retention at faster rates and sluggish kinetics in the high-voltage region. Cr substitution has been shown to enhance electrochemical performance for better Li-ion diffusion and reaction reversibility.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Allison Wustrow, Guanglong Huang, Matthew J. McDermott, Daniel O'Nolan, Chia-Hao Liu, Gia Thinh Tran, Brennan C. McBride, Shyam S. Dwaraknath, Karena W. Chapman, Simon J. L. Billinge, Kristin A. Persson, Katsuyo Thornton, James R. Neilson
Summary: The study identified a cooperative effect in solid-state metathesis reactions that involves using alkaline earth metals instead of alkali metals to lower the formation temperature of orthorhombic YMnO3. Experiments showed that by reacting MgMn2O4 and CaMn2O4 with YOCl in a cooperative cometathesis reaction, reaction temperatures can be reduced to 550°C while maintaining phase selectivity. This approach also showed potential in synthesizing other metastable targets such as TbMnO3, ErMnO3, and DyMnO3 with reduced temperatures and preserved reaction selectivity.
CHEMISTRY OF MATERIALS
(2021)
Article
Materials Science, Multidisciplinary
M. Trini, S. De Angelis, P. S. Jorgensen, P. Hendriksen, K. Thornton, M. Chen
Summary: This study validates the role of contact angle on microstructural evolution during Ni coarsening using a phase-field model, with an equilibrium contact angle of 120 degrees showing the best match to experimental results.
Article
Materials Science, Multidisciplinary
Guanglong Huang, Mojue Zhang, David Montiel, Praveen Soundararajan, Yusu Wang, Jonathan J. Denney, Adam A. Corrao, Peter G. Khalifah, Katsuyo Thornton
Summary: Computational modeling plays a crucial role in experimental design, but accurate input parameters are essential for reliable predictions. A machine learning approach is proposed to extract uncertain or unknown parameters indirectly, refining their range iteratively based on sampling simulations until convergence. The method successfully determines physical parameters for temperature profiles in a high-temperature crystal growth furnace, demonstrating its applicability and accuracy.
COMPUTATIONAL MATERIALS SCIENCE
(2021)
Article
Multidisciplinary Sciences
Kate L. M. Elder, W. Beck Andrews, Markus Ziehmer, Nadiia Mameka, Christoph Kirchlechner, Anton Davydok, Jean-Sebastien Micha, Alexander F. Chadwick, Erica T. Lilleodden, Katsuyo Thornton, Peter W. Voorhees
Summary: The study investigates the formation of grain boundaries during coarsening of nanoporous gold, with a focus on particle detachment and reattachment processes. The development of new grain boundaries is found to be highly dependent on the volume fraction and homogeneity of the nanostructure.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Andrew L. Davis, Vishwas Goel, Daniel W. Liao, Mark N. Main, Eric Kazyak, John Lee, Katsuyo Thornton, Neil P. Dasgupta
Summary: The study found that the rate capability of composite electrodes in solid-state batteries is often limited, with factors including electrostatic potential and solid-state diffusion. Model systems of graphite/Li6PS5Cl composite electrodes can help researchers understand these limiting factors.
ACS ENERGY LETTERS
(2021)
Article
Materials Science, Multidisciplinary
M. J. Higgins, J. Kang, G. Huang, D. Montiel, N. Lu, H. Liu, Y. F. Shen, P. Staublin, J. S. Park, J. D. Almer, P. Kenesei, P. G. Sanders, R. M. Suter, K. Thornton, A. J. Shahani
Summary: A study reported a mode of grain growth where grain centers undergo macroscopic translations during nonisothermal annealing. It was found that dissolution of semicoherent precipitates generated dislocations, increasing the stored strain energy within grains. Grains showed unexpected translations over length scales of 10-100 μm, as revealed by phase-field simulations in strain-energy-driven grain growth.
PHYSICAL REVIEW MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Hanlei Zhang, Hao Liu, Louis F. J. Piper, M. Stanley Whittingham, Guangwen Zhou
Summary: This article reviews recent progress in understanding the phenomena of oxygen loss and the resulting structural degradation in layered oxide cathodes. The major driving forces and associated structural degradation resulting from oxygen loss are presented. The kinetic pathways enabling oxygen loss and the resulting electrochemical fade are discussed, along with possible approaches to mitigate oxygen loss and novel analytical methods for probing oxygen loss.
Article
Nanoscience & Nanotechnology
Qinglu Fan, Mateusz Jan Zuba, Yanxu Zong, Ashok S. Menon, Anthony T. Pacileo, Louis F. J. Piper, Guangwen Zhou, Hao Liu
Summary: The surface structure and chemistry of the layered transition metal oxide cathode play a crucial role in its function and degradation. Modification of the surface using a chemical reduction method can improve the long-term capacity retention but compromise the rate capability.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Rebecca D. McAuliffe, Guanglong Huang, David Montiel, Apurva Mehta, Ryan C. Davis, Victoria Petrova, Katie L. Browning, James R. Neilson, Ping Liu, Katsuyo Thornton, Gabriel M. Veith
Summary: A paradigm for studying complex reaction mechanisms in material synthesis was highlighted. The use of thin-film bilayers provided a simplified system to study solid-state metathesis reactions and revealed the complexity of diffusion at solid-state interfaces.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Gabrielle E. Kamm, Guanglong Huang, Simon M. Vornholt, Rebecca D. McAuliffe, Gabriel M. Veith, Katsuyo S. Thornton, Karena W. Chapman
Summary: The article discusses the importance of understanding and controlling the phenomena that limit solid-state reactions for material synthesis. The study focuses on a model reaction and explores how altering the packing and interfacial contact between reagent particles affects the reaction kinetics. Analysis shows that there are different kinetic regimes in the reaction process, with the fast kinetic regime dominating the initial stages of the reaction. The article also presents simulation results that support the observed experimental findings.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Jiwei Wang, Grayson Hoteling, Robert Shepard, Matthew Wahila, Fei Wang, Manuel Smeu, Hao Liu
Summary: In this study, the structure features of the Co3+/Co2+ redox couple in Na2-xCoSiO4 phases were elucidated using high-resolution synchrotron X-ray diffraction and X-ray pair distribution function analysis. The results indicate that the formation of modulated structures is induced by Na+/vacancy and Co2+/Co3+ charge orderings, which is crucial for understanding the function and performance of sodium transition metal silicate electrodes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Vishwas Goel, Kuan-Hung Chen, Neil P. Dasgupta, Katsuyo Thornton
Summary: In this study, continuum-scale modeling is used to optimize the architecture of Highly Ordered Laser-patterned Electrodes (HOLE) for fast-charging of Li-ion batteries. The parameterization of the model is performed using an automated procedure based on the particle swarm optimization algorithm. The results show that there exists an optimal spacing for the HOLE architecture, below which the marginal gain in performance decreases rapidly.
ENERGY STORAGE MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Vishwas Goel, Yanjun Lyu, Stephen DeWitt, David Montiel, Katsuyo Thornton
Summary: This paper reviews existing simulation tools for simulating microgalvanic corrosion during free immersion. It introduces a recently developed application that uses PRISMS-PF, an open-source phase-field modeling framework, to account for electrochemical reactions and ionic migration in determining the evolution of corrosion front. The paper also demonstrates the capability of the application by simulating corrosion of the matrix phase of an alloy near a secondary phase particle in two and three dimensions.
MRS COMMUNICATIONS
(2022)